CN105948280A - Anaerobic biological oxidation water pollution remediation method with Fe3+ in hematite as electron acceptor - Google Patents
Anaerobic biological oxidation water pollution remediation method with Fe3+ in hematite as electron acceptor Download PDFInfo
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- CN105948280A CN105948280A CN201610586374.5A CN201610586374A CN105948280A CN 105948280 A CN105948280 A CN 105948280A CN 201610586374 A CN201610586374 A CN 201610586374A CN 105948280 A CN105948280 A CN 105948280A
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F3/00—Biological treatment of water, waste water, or sewage
- C02F3/34—Biological treatment of water, waste water, or sewage characterised by the microorganisms used
- C02F3/341—Consortia of bacteria
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F3/00—Biological treatment of water, waste water, or sewage
- C02F3/28—Anaerobic digestion processes
- C02F3/2806—Anaerobic processes using solid supports for microorganisms
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2103/00—Nature of the water, waste water, sewage or sludge to be treated
- C02F2103/06—Contaminated groundwater or leachate
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2305/00—Use of specific compounds during water treatment
- C02F2305/06—Nutrients for stimulating the growth of microorganisms
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Abstract
The invention discloses an anaerobic biological oxidation water pollution remediation method with Fe3+ in hematite as an electron acceptor. According to the method, Fe3+ in hematite serves as the electron acceptor and is loaded with functional microbial florae, and reduction-state pollutants in water are subjected to oxidation removal in the anaerobic or anoxic environment, wherein functional microorganisms include Geobacter sulfurreducens and Shewanella spp.. The method is wide in application range, low in cost, ideal in effect and especially suitable for remediating polluted water with high remediation difficulty.
Description
Technical field
The present invention relates to a kind of water pollution remediation technology, relate more specifically to a kind of with Fe in bloodstone3+Anaerobic biological oxidation water pollution amelioration method for electron acceptor.
Background technology
Traditional water pollution remediation technology is by artificial aeration, high-level oxidation technology or adds cleaning up material etc. and repairs subsoil water, its investment, runs and maintenance cost is higher.Therefore, filter out and be applicable to water and pollute the native electron receptor of anaerobic biological oxidation recovery technique, develop economy, effective, feasible anaerobic biological oxidation recovery technique significant.
The most ancient life process microbiological anaerobic oxidation, can make water pollution oxidation recovery technique to be no longer necessary to artificial aeration, adds oxidant (Fenton reagent, persulfate slow releasing agent etc.) or add oxygen-release material (ORC), thus be substantially reduced cost of sewage disposal.
Ammonia nitrogen is more typical in water body and is distributed relatively broad reduction-state pollutant.Ammoxidation process is a key link of nature nitrogen cycle, directly influences the generation of nitrate, nitrous oxide and nitrogen.Having research to point out, in sea water and freshwater environment, the nitrogen of 67% generates and is derived from anaerobic ammonium oxidation process Anammox (NH4 +By NO2 +Oxidation i.e. Anammox, along with the process of nitrate reductase).But, terrestrial ecosystems there is also anaerobic ammonium oxidation process, i.e. Feammox (NH equally4 +By Fe3+The process of oxidation), mineralized nitrogen can be nitrite along with Fe by this process3+Reduction.
The composition of some organic contamination places COD mainly includes methane, volatile fatty acid, biodegradable organic compounds (fulvic acid and humic acid) and other reduction-state compounds.About the existing correlational study of underground water pollution COD and the recovery technique of ammonia nitrogen and repair materials, wherein correlated response material mainly includes Zero-valent Iron, Zero-valent Iron-activated carbon-modified alta-mud, Zero-valent Iron-zeolite-oxygen-release material, clinoptilolite-activated carbon, clay-iron chloride mud.COD and ammonia nitrogen are removed by these repair materials mostly by physical-chemical reaction process, and when physical reactions reaches balance, the pollutant being adsorbed onto material surface exist secondary release risk, and chemical reactions at the same time is difficult to thorough for pollutant innoxious removal.
At present with Fe3+Anaerobic biological oxidation process study for electron acceptor launches around the nitrogen cycle mechanism in terrestrial ecosystems mostly, and is used mostly hydrated ferric oxide (ferrihydrite), goethitum, lepidocrocite, iron chloride, ferric citrate as electron acceptor.But these materials or chemical property are not sufficiently stable, or the distribution in nature is extensive not, and these factors the most indirectly make the popularization and application feasibility of this technology be deteriorated or cost is increased.
Summary of the invention
In view of this, it is an object of the invention to provide a kind of method using new material to carry out anaerobic biological oxidation water pollution amelioration as electron acceptor, be specially a kind of with Fe in bloodstone3+Anaerobic biological oxidation water pollution amelioration method for electron acceptor.The method applied range of the present invention, with low cost, satisfactory for result, it is particularly suited for repairing the polluted-water (such as underground water pollution) that difficulty is bigger.
For achieving the above object, the present invention provides a kind of with Fe in bloodstone3+For the anaerobic biological oxidation water pollution amelioration method of electron acceptor, it is with the Fe in bloodstone3+For electron acceptor, loading functional microorganism species, under anaerobism or anaerobic environment, the reduction-state pollutant in water are carried out oxidation removal；
Wherein, described functional microorganism includes ground bacillus (Geobacter sulfurreducens) and Shewanella (Shewanella spp.).
Described bloodstone is that this area is conventional, and the most in general, its chemical composition is α-Fe2O3, crystal belongs to trigonal system.Preferably, described bloodstone is graininess, and particle diameter is more than 1mm, and concrete particle size determines according to the hydraulics in practical application engineering, in case locking system blocking.
In being embodied as, the present invention with Fe in bloodstone3+Following steps are preferably included for the anaerobic biological oxidation water pollution amelioration method of electron acceptor:
1) in hermetic container, with the functional microorganism engineering bacteria immersion bubble bloodstone of activation；
2) nitrogen 10-15min it is filled with, constant temperature culture at 33-37 DEG C, until ammonia nitrogen, COD concentration in hermetic container reduce by more than 90%, engineering bacterium solution is emptied；
3), after using normal saline to soak the biomembranous bloodstone 20-40min of load, normal saline is emptied；
4) step 3 is repeated) after 2-3 time, the filling of biomembranous bloodstone will be loaded with to sewage treatment unit, under anaerobism or anaerobic environment, the reduction-state pollutant in water will be carried out oxidation removal.
Described normal saline is described in the routine of this area, it is preferable that described normal saline is 0.85%NaCl solution.
Preferably, the mass ratio of described ground bacillus (Geobacter sulfurreducens) and Shewanella (Shewanella spp.) preferred engineering bacterium solution in use is 1:1.5～1.5:1, more preferably 1:1.
The culture medium cultivating described functional microorganism can be that this area is conventional, it is preferable that described culture medium includes: 0.535g/L NH4Cl, 0.136g/L KH2PO4, 0.204g/L MgCl2·6H2O, 0.147g/L CaCl2·2H2O, 2.52g/L NaHCO3, 0.82g/L CH3COONa, 0.735g/L ferric citrate, 1mL/L trace element mixed solution, and 1mL/L vitamin mixed solution.
Wherein, described trace element mixed solution, as described in the routine of this area, preferably includes 0.1g/L CoCl2·6H2O、0.425g/L MnCl2·4H2O、0.05g/L ZnCl2、0.01g/L NiCl2·6H2O、0.015g/L CuSO4·5H2O、0.01g/L Na2MoO42H2O and 0.01g/L Na2SeO4·2H2O.Described vitamin mixed solution as described in the routine of this area, the preferably mixed solution of vitamin B1, B2 and B5.
Generally, conventional by this area, described functional microorganism is seeded in described culture medium, normal condition is cultivated activation and i.e. be can be used for the load biofilm of bloodstone.
Fe in described bloodstone3+Reduction product Fe2+Can be again as the electron donor of bioreduction process, the oxidation state pollutant in further biodegradation water body (such as nitrate, sulfate, chlorinated compound, Cr (VI) etc.) under anaerobic environment.
With Fe in bloodstone3+For the biooxidation products nitrate of electron acceptor, sulfate, chlorinated compound, Cr (VI) etc., may participate in reduction product Fe2+Bioprocesses for electron donor, it is possible to enter next stage with sulfur (S), troilite (FeS2), solid organic carbon source etc. be electron donor biological respinse unit.
The present invention achieves following beneficial effect:
Ground bacillus (Geobacter sulfurreducens) and Shewanella (Shewanella spp.) are loaded bloodstone, under anaerobism or anaerobic environment, the reduction-state pollutant in water are carried out oxidation removal by the present invention, experiment shows that contaminant removal efficiency is high, COD and ammonia nitrogen removal frank are up to more than 90%, with low cost, easy to operate, have a good application prospect.
Accompanying drawing explanation
Fig. 1 shows that the present invention is with Fe in bloodstone3+Principle for the anaerobic biological oxidation water pollution amelioration method of electron acceptor；
Fig. 2 is the removal efficiency comparing result figure of experimental group and matched group COD in embodiment 1, and wherein, two, top curve is respectively the data of 1# and 2# control experiment, and two, lower section curve is respectively the data of 1# and 2# experimental group biological restoration；
Fig. 3 is the removal efficiency comparing result figure of experimental group and matched group ammonia nitrogen in embodiment 2, and wherein, lower curve is the data of experimental group biological restoration, and top curve is the data of control experiment.
Detailed description of the invention
For making the object, technical solutions and advantages of the present invention clearer, below in conjunction with specific embodiment, and referring to the drawings, the present invention is described in further detail.
The present invention provide with Fe in bloodstone3+Operation principle for the anaerobic biological oxidation water pollution remediation technology of electron acceptor is:
As it is shown in figure 1, the restorative procedure of the present invention is with the Fe in bloodstone3+For electron acceptor, loading functional microorganism species (includes ground bacillus-Geobacter sulfurreducens and Shewanella-Shewanella spp.), under anaerobism or anaerobic environment, the reduction-state pollutant (such as ammonia nitrogen, COD, benzene homologues, As (III) etc.) in water is carried out oxidation removal.Fe in bloodstone3+Reduction product Fe2+Again as the electron donor of Anaerobe reduction reaction process, thus the oxidation state pollutant (such as nitrate, sulfate, chlorinated compound, Cr (VI) etc.) in water body can be removed further.
More specifically, the present invention with Fe in bloodstone3+For the anaerobic biological oxidation water pollution amelioration method of electron acceptor, wherein said hematization studies and is divided into α-Fe2O3, crystal belongs to the oxide of trigonal system, is the essential mineral form of ferrum oxide.Described bloodstone is graininess, and particle diameter is more than 1mm, and concrete particle size determines according to the hydraulics in practical application engineering, in case locking system blocking.
In following specific embodiment, microorganism used therefor is purchased from Chinese Typical Representative Organism Depositary (CCTCC), is used for loading biofilm after activation is cultivated with domestication.
Embodiment 1
With the treatment of advanced stage landfill leachate of Beijing city refuse landfill for process object, after suitably dilution, COD concentration is about 600mg/L, pH is 8.30, and ORP is-436mV, and EC is 24.4mS/cm.
The method using the present invention processes, specifically:
1) activate, tame function microorganism ground bacillus (Geobacter sulfurreducens) and Shewanella (Shewanella spp.)；
The culture medium cultivating described functional microorganism includes: 0.535g/L NH4Cl, 0.136g/L KH2PO4, 0.204g/L MgCl2·6H2O, 0.147g/L CaCl2·2H2O, 2.52g/L NaHCO3, 0.82g/L CH3COONa, 0.735g/L ferric citrate, 1mL/L trace element mixed solution, and 1mL/L vitamin mixed solution；Described trace element mixed solution includes 0.1g/L CoCl2·6H2O、0.425g/L MnCl2·4H2O、0.05g/L ZnCl2、0.01g/L NiCl2·6H2O、0.015g/L CuSO4·5H2O、0.01g/L Na2MoO4·2H2O and 0.01g/L Na2SeO4·2H2O；Described vitamin mixed solution is the mixed solution of vitamin B1, B2 and B5；Wherein the mass ratio of bacillus (Geobacter sulfurreducens) and Shewanella (Shewanella spp.) engineering bacterium solution in use is 1:1；
Select bloodstone granule (particle diameter 2-4mm) as electron acceptor, in hermetic container, steep bloodstone with the engineering bacteria immersion of activation；
2), before reaction starts, it is filled with 10min nitrogen, to ensure anaerobic reaction environment, constant temperature culture at 33-37 DEG C, until ammonia nitrogen, COD concentration in hermetic container reduce by more than 90%, engineering bacterium solution is emptied；
3), after using 0.85%NaCl solution soaking to load biomembranous bloodstone 20-40min, normal saline is emptied；
4) step 3 is repeated) after 2-3 time, the filling of biomembranous bloodstone will be loaded with to sewage treatment unit, under anaerobism or anaerobic environment, the reduction-state pollutant in water will be carried out oxidation removal.
For contrasting the treatment effect of the inventive method, 1 group of contrast test (matched group) is set, in reaction system, i.e. adds a certain amount of NaN3Carry out sterilizing, to ensure the gnotobasis in reaction system, it was demonstrated that the effect of function microorganism in the inventive method.
Result: anaerobic reaction is after 50 days, in reaction system rest COD concentration be 50mg/L, COD clearance be 91.67%.And contrast test group (physics chemical action), COD concentration is 500mg/L, and COD clearance is only 16.67%, and concrete data are as shown in Figure 2.
Embodiment 2
With certain generted address water for processing object, principal character pollutant are ammonia nitrogen, and its initial concentration is 16mg N L-1。
The method using the present invention processes, specifically:
1) activate, tame function microorganism ground bacillus (Geobacter sulfurreducens) and Shewanella (Shewanella spp.)；
The culture medium cultivating described functional microorganism includes: 0.535g/L NH4Cl, 0.136g/L KH2PO4, 0.204g/L MgCl2·6H2O, 0.147g/L CaCl2·2H2O, 2.52g/L NaHCO3, 0.82g/L CH3COONa, 0.735g/L ferric citrate, 1mL/L trace element mixed solution, and 1mL/L vitamin mixed solution；Described trace element mixed solution includes 0.1g/L CoCl2·6H2O、0.425g/L MnCl2·4H2O、0.05g/L ZnCl2、0.01g/L NiCl2·6H2O、0.015g/L CuSO4·5H2O、0.01g/L Na2MoO4·2H2O and 0.01g/L Na2SeO4·2H2O；Described vitamin mixed solution is the mixed solution of vitamin B1, B2 and B5；Wherein the mass ratio of bacillus (Geobacter sulfurreducens) and Shewanella (Shewanella spp.) engineering bacterium solution in use is 1:1.2；
Select bloodstone granule (particle diameter 2-4mm) as electron acceptor, in hermetic container, steep bloodstone with the engineering bacteria immersion of activation；
2), before reaction starts, it is filled with 15min argon, to ensure anaerobic reaction environment, constant temperature culture at 33-37 DEG C, until ammonia nitrogen, COD concentration in hermetic container reduce by more than 90%, engineering bacterium solution is emptied；
3), after using 0.85%NaCl solution soaking to load biomembranous bloodstone 20-40min, normal saline is emptied；
4) step 3 is repeated) after 2-3 time, the filling of biomembranous bloodstone will be loaded with to sewage treatment unit, under anaerobism or anaerobic environment, the reduction-state pollutant in water will be carried out oxidation removal.
For contrasting the treatment effect of the inventive method, contrast test (matched group) is set, in reaction system, i.e. adds a certain amount of NaN3Carrying out sterilizing, to ensure the gnotobasis in reaction system, it was demonstrated that the effect of function microorganism in the inventive method, the present embodiment has carried out two groups of parallel laboratory tests and two groups of parallel control groups experiments simultaneously.
Result: anaerobic reaction is after 29 days, and in biological respinse system, residue ammonia nitrogen concentration is 0.5mg N/L, and clearance is 96.87%.And contrast test group (physics chemical action), ammonia nitrogen concentration is 15.51mg N/L, and clearance is only 16.67%, and concrete data are as shown in Figure 3.
From the result of above-described embodiment it can be seen that the functional microorganism flora that the present invention uses is combined bloodstone has the effect of excellence for repairing polluted-water under anaerobic environment and simple to operate, with low cost, therefore have a good application prospect.
Particular embodiments described above; the purpose of the present invention, technical scheme and beneficial effect are further described; it it should be understood that; the foregoing is only the specific embodiment of the present invention; it is not limited to the present invention; all within the spirit and principles in the present invention, any modification, equivalent substitution and improvement etc. done, should be included within the scope of the present invention.
Claims (8)
1. one kind with Fe in bloodstone3+For the anaerobic biological oxidation water pollution amelioration method of electron acceptor,
It is characterized in that, it is with the Fe in bloodstone3+For electron acceptor, loading functional microorganism species,
Under anaerobism or anaerobic environment, the reduction-state pollutant in water are carried out oxidation removal；
Wherein, described functional microorganism includes ground bacillus (Geobacter sulfurreducens) and wishes
Watt Salmonella (Shewanella spp.).
The most according to claim 1 with Fe in bloodstone3+Anaerobe oxygen for electron acceptor
Changing water pollution amelioration method, it is characterised in that described bloodstone is graininess, particle diameter is more than 1mm.
The most according to claim 1 with Fe in bloodstone3+Anaerobe oxygen for electron acceptor
Change water pollution amelioration method, it is characterised in that comprise the steps:
1) in hermetic container, with the functional microorganism engineering bacteria immersion bubble bloodstone of activation；
2) nitrogen 10-15min it is filled with, constant temperature culture at 33-37 DEG C, until the ammonia in hermetic container
Nitrogen, COD concentration reduce by more than 90%, engineering bacterium solution are emptied；
3) after using normal saline to soak the biomembranous bloodstone 20-40min of load, by normal saline
Emptying；
4) step 3 is repeated) after 2-3 time, the filling of biomembranous bloodstone will be loaded with to sewage disposal
Reduction-state pollutant in water are carried out oxidation removal under anaerobism or anaerobic environment by unit.
The most according to claim 3 with Fe in bloodstone3+Anaerobe oxygen for electron acceptor
Change water pollution amelioration method, it is characterised in that described normal saline is 0.85%NaCl solution.
5. according to according to any one of claim 1-4 with Fe in bloodstone3+Detesting for electron acceptor
Oxygen biological oxidation water pollution amelioration method, it is characterised in that described ground bacillus (Geobacter
And the quality of Shewanella (Shewanella spp.) engineering bacterium solution in use sulfurreducens)
Ratio is 1:1.5～1.5:1, more preferably 1:1.
The most according to claim 1 with Fe in bloodstone3+Anaerobe oxygen for electron acceptor
Change water pollution amelioration method, it is characterised in that the culture medium cultivating described functional microorganism includes: 0.535
g/L NH4Cl, 0.136g/L KH2PO4, 0.204g/L MgCl2·6H2O, 0.147g/L CaCl2·2H2O,
2.52g/L NaHCO3, 0.82g/L CH3COONa, 0.735g/L ferric citrate, 1mL/L trace
Element mixed solution, and 1mL/L vitamin mixed solution.
The most according to claim 6 with Fe in bloodstone3+Anaerobe oxygen for electron acceptor
Change water pollution amelioration method, it is characterised in that described trace element mixed solution includes 0.1g/L
CoCl2·6H2O、0.425g/L MnCl2·4H2O、0.05g/L ZnCl2、0.01g/L NiCl2·6H2O、
0.015g/L CuSO4·5H2O、0.01g/L Na2MoO4·2H2O and 0.01g/L Na2SeO4·2H2O。
The most according to claim 6 with Fe in bloodstone3+Anaerobe oxygen for electron acceptor
Change water pollution amelioration method, it is characterised in that described vitamin mixed solution is vitamin B1, B2
Mixed solution with B5.
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